High‐Performance Al–S Batteries by Spin Polarization Modulation via Catalytic Ni‐MoS2 Nanosheets

Liu, Xiaoya; Liu, Xingjun; Zhan, Jiqiang; Yuan, Wang; Zhu, Yue; Huang, Weiyuan; Li, Hongpeng; Liu, Tongchao; Amine, Khalil; Li, Hongsen; Yu, Guihua

doi:10.1002/anie.202503835

High‐Performance Al–S Batteries by Spin Polarization Modulation via Catalytic Ni‐MoS₂ Nanosheets

Journal Article · Fri May 09 00:00:00 EDT 2025 · Angewandte Chemie International Edition

DOI:https://doi.org/10.1002/anie.202503835· OSTI ID:2588472

Liu, Xiaoya ^[1]; Liu, Xingjun ^[1]; Zhan, Jiqiang ^[1]; Yuan, Wang ^[1]; Zhu, Yue ^[2]; Huang, Weiyuan ^[3]; Li, Hongpeng ^[4]; Liu, Tongchao ^[3]; Amine, Khalil ^[3]; Li, Hongsen ^[1]; Yu, Guihua ^[5]

Qingdao University (China)
University of Texas, Austin, TX (United States); Ocean University of China, Qingdao (China)
Argonne National Laboratory (ANL), Argonne, IL (United States)
Yangzhou University, Jiangsu (China)
University of Texas, Austin, TX (United States)

Aluminum–sulfur (Al–S) batteries catalysts with adsorption and catalytic capabilities can effectively improve the slow redox kinetics, but the current research often ignores the effect of optimizing the electronic structure of the catalyst on improving charge transfer and adsorption. Here, in this study, Ni-doped monolayer MoS₂ nanosheets are synthesized and used as a catalytic additive for the sulfur cathode. The addition of Ni promotes spin splitting of 4d orbital of Mo, thereby affecting polarization degree of the basal plane sulfur and making it change from a low spin state to a high spin one. This high spin configuration raises the electron energy level and provides an active electron state to react with aluminum polysulfides (AlPSs), which optimizes the adsorption energy. At the same time, it accelerates electron transfer and lowers the energy barrier for the overall conversion of the polysulfides. Benefiting from these features, Al–S batteries based on rationally designed S@Ni-MoS₂/C cathodes exhibit a high initial capacity (1603.0 mAh g⁻¹ at 0.5 A g⁻¹) and extraordinary cycling stability (0.035% capacity decay rate during 2000 cycles). This study showcases a spin-polarized electronic structure control strategy to enhance catalytic activity, providing a viable approach for developing efficient catalysts for practical Al–S batteries.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: National Natural Science Foundation of China (NSFC); Robert A. Welch Foundation; USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: AC02-06CH11357; SC0012704

OSTI ID:: 2588472

Journal Information:: Angewandte Chemie International Edition, Journal Name: Angewandte Chemie International Edition Journal Issue: 29 Vol. 64; ISSN 1521-3773; ISSN 1433-7851

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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